JPS61128409A - Dielectric ceramic composition - Google Patents
Dielectric ceramic compositionInfo
- Publication number
- JPS61128409A JPS61128409A JP59250798A JP25079884A JPS61128409A JP S61128409 A JPS61128409 A JP S61128409A JP 59250798 A JP59250798 A JP 59250798A JP 25079884 A JP25079884 A JP 25079884A JP S61128409 A JPS61128409 A JP S61128409A
- Authority
- JP
- Japan
- Prior art keywords
- ceramic composition
- dielectric ceramic
- dielectric
- dielectric constant
- temperature
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G4/00—Fixed capacitors; Processes of their manufacture
- H01G4/002—Details
- H01G4/018—Dielectrics
- H01G4/06—Solid dielectrics
- H01G4/08—Inorganic dielectrics
- H01G4/12—Ceramic dielectrics
- H01G4/1209—Ceramic dielectrics characterised by the ceramic dielectric material
- H01G4/1254—Ceramic dielectrics characterised by the ceramic dielectric material based on niobium or tungsteen, tantalum oxides or niobates, tantalates
- H01G4/1263—Ceramic dielectrics characterised by the ceramic dielectric material based on niobium or tungsteen, tantalum oxides or niobates, tantalates containing also zirconium oxides or zirconates
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/495—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on vanadium, niobium, tantalum, molybdenum or tungsten oxides or solid solutions thereof with other oxides, e.g. vanadates, niobates, tantalates, molybdates or tungstates
- C04B35/497—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on vanadium, niobium, tantalum, molybdenum or tungsten oxides or solid solutions thereof with other oxides, e.g. vanadates, niobates, tantalates, molybdates or tungstates based on solid solutions with lead oxides
- C04B35/499—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on vanadium, niobium, tantalum, molybdenum or tungsten oxides or solid solutions thereof with other oxides, e.g. vanadates, niobates, tantalates, molybdates or tungstates based on solid solutions with lead oxides containing also titanates
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Ceramic Engineering (AREA)
- Power Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Structural Engineering (AREA)
- Organic Chemistry (AREA)
- Inorganic Insulating Materials (AREA)
- Compositions Of Oxide Ceramics (AREA)
- Ceramic Capacitors (AREA)
Abstract
(57)【要約】本公報は電子出願前の出願データであるた
め要約のデータは記録されません。(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.
Description
【発明の詳細な説明】
(産業上の利用分野)
この発明は、誘電率が8000以上と高く、かつその焼
結温度が900〜1000t:と低いことを特徴とする
誘電体磁器組成物に関する。DETAILED DESCRIPTION OF THE INVENTION (Field of Industrial Application) The present invention relates to a dielectric ceramic composition characterized by having a high dielectric constant of 8000 or more and a low sintering temperature of 900 to 1000 t:.
(従来の技術)
積層セラミックコンデンサは小型で大容毫であること、
高周波特性にすぐれていること、耐熱性にすぐれ、かつ
量産性に富むなどの特徴を有している。したがって、窒
業用電子機器、民生用電子機器の軽薄短小、高品質、高
周波設計などの要求に合致することから近年その需要は
増加の一途をたどっている。(Conventional technology) Multilayer ceramic capacitors are small and large in size;
It has characteristics such as excellent high frequency characteristics, excellent heat resistance, and ease of mass production. Therefore, the demand for it has been increasing in recent years because it meets the demands of industrial electronic equipment and consumer electronic equipment such as lightness, thinness, compactness, high quality, and high frequency design.
従来の積層セラミックコンデンサは、内部電極としCA
u、Pt、Paなど、高価な貴金属を用いるのが一般的
であった。Conventional multilayer ceramic capacitors use internal electrodes and CA
It was common to use expensive noble metals such as u, Pt, and Pa.
(発明が解決しようとする問題)
しかしながら、上記した貴金属を内部1僅とする積層セ
ラミックコンデンサでは、生産コストの過半がシ函材料
費となシ、全体のコスト全低減することに限度があった
。(Problem to be solved by the invention) However, in the above-mentioned multilayer ceramic capacitor with a small amount of precious metal inside, the majority of the production cost is the cost of the box material, so there is a limit to the total reduction of the overall cost. .
このため、チタン酸バリウムを生木とする高d電率系の
磁器組成物に、ホウ素、ビスマス、鉛などの酸化物よ)
なるガラス成分を添加し、焼成温度を従前の1300〜
1550tから1100〜1150Cに低下させ、比較
的安価な銀−パラジウム系合金を内部゛ぺ極とする、低
温i結可能な積層セラミックコンデンナが開発されるに
至った〇しかし、ガラス成分を添加することKより、本
来チタン酸バリウム母体組成が有する誘電率を低減させ
、積層セラミックコンデンサの寸法とし′Cは逆に大き
くなシ、電価材料のコストの低下を打ら消しCしまうと
いう欠点が見られた。For this reason, oxides such as boron, bismuth, lead, etc. are used in high-d electric conductivity porcelain compositions made of raw barium titanate.
By adding a glass component, the firing temperature was increased from 1300 to
A multilayer ceramic capacitor capable of low-temperature curing has been developed, which lowers the temperature from 1550t to 1100-1150C and uses a relatively inexpensive silver-palladium alloy as the internal electrode.However, a glass component is added. Therefore, the dielectric constant originally possessed by the barium titanate matrix composition is reduced, and when the dimensions of the multilayer ceramic capacitor are changed, C becomes large, which cancels out the reduction in the cost of the electrically conductive material. It was done.
(発明の目的)
したがつC1この発明は、上記した従来技術のように#
、[率の低下をもたらすことなく、つまり誘電率の値が
8000以上を示し、かつその焼結温度が900〜10
00でと低い誘電体磁器組成物を提供することを目的と
する◇
また、この発明は、焼結1度が低いことを利用し゛C1
比貌的安渇な銀−パラジウム系合金を内部電極とする積
層セラミックコンデンサを構成する誘電体材料としC利
用可能21−誘電体磁器組成物を提供することを目的と
する。(Object of the invention) However, C1 This invention is similar to the above-mentioned prior art.
, [without causing a decrease in the dielectric constant, that is, the dielectric constant value is 8000 or more, and the sintering temperature is 900 to 10
It is an object of the present invention to provide a dielectric ceramic composition with a low C1
An object of the present invention is to provide a 21-dielectric ceramic composition that can be used as a dielectric material constituting a multilayer ceramic capacitor having a comparatively stable silver-palladium alloy as an internal electrode.
(発明の構成)
この発明にかかる誘電体磁器組成物は、Pb(1)Pb
(Ni1/3Nbx、4)O,、FD’riO,、Pb
(ZraLイW4)O,オよびA(Cu4(Nb%)O
,を主成分とするものである。(Structure of the Invention) The dielectric ceramic composition according to the present invention includes Pb(1)Pb
(Ni1/3Nbx, 4)O,, FD'riO,, Pb
(ZraL-W4)O, O and A(Cu4(Nb%)O
, is the main component.
また、この発明にか力瓢る誘電体磁器組成物は、上記し
た主成分に対し′C1副成分とし゛Cマンガンを添加含
有させたものである。Further, the dielectric ceramic composition useful in the present invention is one in which C manganese is added as a C1 subcomponent to the above-mentioned main component.
上記した主成分は次の組成領域からなるものである。The main components mentioned above consist of the following compositional regions.
つまり、
PI)(Ni電NbzA)0. 45〜75そルチ
PbTL0. 20〜40モルチP
モルZn4W%)Os ・15〜15モルチ
A(Cu’4Nbz4)o、 1.0〜I Q
%ル9g、kcだし、ム(Cu%Nbt4 )O,のム
はBa、 Sr。That is, PI) (Ni conductor NbzA)0. 45-75 Soluchi PbTL0. 20-40 moltiP
Mol Zn4W%)Os ・15~15 Molti A(Cu'4Nbz4)o, 1.0~I Q
It is 9g, KC, and (Cu%Nbt4)O, is Ba and Sr.
およびCaのうち1種を意味する。and Ca.
また、上記した主成分に対し′C1副成分とし°C添加
含有するマンガン量はMnO,に換算し゛Cα5モルチ
以下の範囲にある。Further, the amount of manganese added to the above-mentioned main component as a C1 subcomponent is within the range of Cα5 molti in terms of MnO.
上記した構成成分のうち、主成分の組成範囲を限定した
。rN由は次のとおシである。Among the above-mentioned components, the composition range of the main components was limited. The reason for rN is as follows.
第1K1Pb(Ni電It)≠p、につぃで、45モル
チ未膚になると誘電率か8000未満になるとともに、
誘電正接が2.5俤を越える。一方、75モモルを壇え
ると誘電率の低下が著しくなりaoo。1st K1Pb (Ni electric It) ≠ p, when the temperature becomes 45 molar, the dielectric constant becomes less than 8000, and
The dielectric loss tangent exceeds 2.5 t. On the other hand, when 75 momoles are added, the dielectric constant decreases significantly.
未溝となる。It becomes ungrooved.
M2に、Pl)TiOsについCl2oモルチ未満にさ
ると誘電率の低下が著しくなシ5ooo未満と表る。一
方、40モル憂を4えると誘電率が8000未満になる
とともに誘電正接が2.5チを越える。When M2 is less than Cl2o, the dielectric constant of Pl)TiOs decreases significantly, which is less than 5ooo. On the other hand, when 40 moles are increased by 4, the dielectric constant becomes less than 8000 and the dielectric loss tangent exceeds 2.5.
第3に、Pb(Zn%W’()OsKつい乙 Q、5%
未膚になると焼成温度が1000″Cを越え、誘電率が
8000未イi々となる。一方、1°5−r:ルチを」
えると焼成温度は900C以下に低下するが、誘電率が
8000未情になるとともに、比抵抗も室温で1o11
Ω、−1に達しなくなる。 ′
第4に、ム(Cu% N I) !/” )’s K
ライ’C%t Oモルチ未満になると、焼成温度が10
01t−”4える。Third, Pb(Zn%W'()OsKQ, 5%
When it becomes loose, the firing temperature exceeds 1000"C and the dielectric constant becomes less than 8000. On the other hand, 1°5-r: ruti"
As the temperature increases, the firing temperature drops to below 900C, but the dielectric constant becomes 8000, and the resistivity also decreases to 1o11 at room temperature.
Ω, no longer reaches -1. 'Fourthly, MU (Cu% N I)! /” )'s K
When the Li'C%t is less than O morch, the firing temperature is 10%
01t-"4 get.
一方、10モル慢を越えると誘電率が8000未満に低
下するとともに比抵抗が10”Q−cmに達しなくなる
。On the other hand, when the molar ratio exceeds 10, the dielectric constant decreases to less than 8,000 and the resistivity does not reach 10''Q-cm.
また、主成分に対するマンガン量がMnotK換算し゛
C005モル慢を越えると、室温での比抵抗が1014
Ω、鴬に達しなくなる。In addition, if the amount of manganese relative to the main component exceeds ゛C005 molar equivalent in terms of MnotK, the specific resistance at room temperature will be 1014
Ω, it won't reach Umugi.
(効果)
この発明にかかる誘電体磁器組成物は、次のような効果
を有する。(Effects) The dielectric ceramic composition according to the present invention has the following effects.
■ 誘電率(g)が8000以上の直を示す。■ Exhibits a dielectric constant (g) of 8000 or more.
■ 誘電正接(t4nδ)がZSLs以下である。■ The dielectric loss tangent (t4nδ) is less than or equal to ZSLs.
■ 室温では比抵抗が10”n、m以上である。■ Specific resistance is 10"n,m or more at room temperature.
■ 焼結温度が900〜100C1’と低い。■Sintering temperature is low at 900-100C1'.
■ マンガンを含有させることによシ、室温および高温
(ast’)での比抵抗が10’Ω、為以上に改善され
る。(2) By incorporating manganese, the specific resistance at room temperature and high temperature (ast') is improved by more than 10'Ω.
したがつC1この発明にかかる誘電体磁器組成物は一般
の磁3コンデンサのみならず、積層セラミックコンデン
サの誘電材料とし゛C使用可能なものである。特に、積
層セラミックコンデンサを製造する場合、焼結温度が低
^ことに起因し′C1内部・Ef&とし゛C銀−パラジ
ウム系材料を用いることができ、小型、大容量のものを
工業的に生産することができる。Therefore, the dielectric ceramic composition according to the present invention can be used as a dielectric material not only for general magnetic 3 capacitors but also for multilayer ceramic capacitors. In particular, when manufacturing multilayer ceramic capacitors, due to the low sintering temperature, silver-palladium materials can be used for the inside of C1 and Ef, making it possible to industrially produce small-sized, large-capacity capacitors. be able to.
(実施列)
以下、この発明を実施例に従つ゛C詳細に説明すTo、
、cuoおよびMnO,を出発原料とし、第1表に示す
組成比の磁器組成物が最終的に得られるように各原料を
秤量した。各秤量原料を100gとし、ポリエチレン製
ポットにメノウ玉石とともに入れ、10時時間式混合し
た。混合カスラリ−を脱水、乾燥し、アルミナ質の匣に
入れ、650〜800Cで2時間保持し°C仮焼し、−
次反応粉末(仮焼粉末)を得た。仮焼粉末をあらかじめ
粗粉砕し、バインダーとし゛Cポリビニルアルコールを
3ffit%加えC再び湿式混合粉砕を行った。得られ
たスラリーを乾燥したのち、50メツシユの篩を通し′
C成形用整粒扮粉末した。次いで、オイルプレスで20
00hF/dの圧力で直径12四、厚み1.28の円板
状に成形加工した。成形円板をジルコニア質の匣に入れ
、適度の鉛雰囲気に設定し九逍気炉内で、850〜11
00rの温度で2時間焼成した。(Implementation sequence) This invention will be described in detail below according to examples.
, cuo, and MnO were used as starting materials, and each raw material was weighed so as to finally obtain a ceramic composition having the composition ratio shown in Table 1. 100 g of each raw material was weighed, placed in a polyethylene pot together with agate boulders, and mixed for 10 hours. The mixed cast slurry was dehydrated, dried, placed in an alumina box, held at 650-800C for 2 hours, and calcined at -
A next reaction powder (calcined powder) was obtained. The calcined powder was coarsely pulverized in advance, 3 ffit% of polyvinyl alcohol was added as a binder, and wet mixing and pulverization was performed again. After drying the resulting slurry, it was passed through a 50 mesh sieve.
C was made into a sized powder for molding. Next, use an oil press for 20
It was molded into a disk shape with a diameter of 124 mm and a thickness of 1.28 mm at a pressure of 00 hF/d. The molded disk was placed in a zirconia box, set to an appropriate lead atmosphere, and heated to 850 to 11
It was baked at a temperature of 00 r for 2 hours.
得られた磁器円板の両直に、硼硅酸鉛ガラスフリットを
含む銀ペーストを塗布し、750Cで10分間焼き付け
゛C電厘を形成し、測定用の試料とした。A silver paste containing a lead borosilicate glass frit was applied on both sides of the obtained porcelain disk, and baked at 750C for 10 minutes to form a C ring, which was used as a sample for measurement.
各試料につき、静電容量(C)、誘電正接(t、nδ)
をYHI’fiLCRメータ4274を用イ゛〔温度2
5c。For each sample, capacitance (C), dielectric loss tangent (t, nδ)
Use YHI'fi LCR meter 4274.
5c.
1KHz、17rmsで測定した。 また、絶縁抵抗(
工R)はタケダ理研製メグオームメータTR8601を
用い、直Rs o □ v印加2分後の値を測定した。Measured at 1KHz and 17rms. In addition, insulation resistance (
(R) was measured using a megohmmeter TR8601 manufactured by Takeda Riken, and the value was measured 2 minutes after direct Rso□v application.
試料の厚み、底玉の直径寸法を測定し、誘電率(ε)お
よび比抵抗(p)を計算し、その信果を第2表に示した
。The thickness of the sample and the diameter of the bottom ball were measured, and the dielectric constant (ε) and specific resistance (p) were calculated, and the results are shown in Table 2.
さらく、各X科の焼成温度を第2表に示した。Furthermore, the firing temperatures for each group X are shown in Table 2.
なお、第1表、第2表中東部を付したものは、この発明
範囲外のものであシ、それ以外のものはこの発明範囲内
のものである。It should be noted that those marked with the middle east part of Table 1 and Table 2 are outside the scope of this invention, and the others are within the scope of this invention.
Claims (2)
3、PbTiO_3、Pb(Zn_1_/_2W_1_
/_2)O_3およびA(Cu_1_/_3Nb_2_
/_3)O_3からなり、それぞれのモル分率が次の範
囲にある、ことを特徴とする誘電本磁器組成物。 Pb(Ni_1_/_3Nb_2_/_3)O_3 4
5〜75モル%PbTiO_3 20〜40モル% Pb(Zn_1_/_2W_1_/_2)O_3 0.
5〜15モル%A(Cu_1_/_3Nb_2_/_3
)O_3 1.0〜10モル%ただし、A(Cu_1_
/_3Nb_2_/_3)O_3のAはBa、Sr、お
よびCaのうち1種。(1) Pb(Ni_1_/_3Nb_2_/_3)O_
3, PbTiO_3, Pb(Zn_1_/_2W_1_
/_2) O_3 and A(Cu_1_/_3Nb_2_
/_3) A dielectric ceramic composition comprising O_3, each having a molar fraction within the following range. Pb(Ni_1_/_3Nb_2_/_3)O_3 4
5-75 mol% PbTiO_3 20-40 mol% Pb(Zn_1_/_2W_1_/_2)O_3 0.
5 to 15 mol% A (Cu_1_/_3Nb_2_/_3
)O_3 1.0 to 10 mol% However, A(Cu_1_
/_3Nb_2_/_3) A in O_3 is one of Ba, Sr, and Ca.
O_3、PbTiO_3、Pb(Zn_1_/_2W_
1_/_2)O_3およびA(Cu_1_/_2Nb_
1_/_2)O_3からなる主成分に対して、マンガン
をMnO_2に換算して0.5モル%以下含有する、こ
とを特徴とする特許請求の範囲第(1)項記載の誘電体
磁器組成物。(2) Said Pb (Ni_1_/_3Nb_2_/_3)
O_3, PbTiO_3, Pb(Zn_1_/_2W_
1_/_2) O_3 and A(Cu_1_/_2Nb_
1_/_2) The dielectric ceramic composition according to claim (1), which contains 0.5 mol% or less of manganese in terms of MnO_2 with respect to the main component consisting of O_3. .
Priority Applications (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59250798A JPS61128409A (en) | 1984-11-27 | 1984-11-27 | Dielectric ceramic composition |
| DE19853541517 DE3541517A1 (en) | 1984-11-27 | 1985-11-23 | DIELECTRIC CERAMIC COMPOSITION |
| CA000496126A CA1251037A (en) | 1984-11-27 | 1985-11-25 | Dielectric ceramic composition |
| US06/801,483 US4601989A (en) | 1984-11-27 | 1985-11-25 | Dielectric ceramic composition |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59250798A JPS61128409A (en) | 1984-11-27 | 1984-11-27 | Dielectric ceramic composition |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS61128409A true JPS61128409A (en) | 1986-06-16 |
Family
ID=17213202
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59250798A Expired - Lifetime JPS61128409A (en) | 1984-11-27 | 1984-11-27 | Dielectric ceramic composition |
Country Status (4)
| Country | Link |
|---|---|
| US (1) | US4601989A (en) |
| JP (1) | JPS61128409A (en) |
| CA (1) | CA1251037A (en) |
| DE (1) | DE3541517A1 (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5439857A (en) * | 1993-06-30 | 1995-08-08 | Murata Manufacturing Co., Ltd. | Dielectric ceramic composition |
Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4753905A (en) * | 1985-07-31 | 1988-06-28 | Murata Manufacturing Co., Ltd. | Dielectric ceramic composition |
| US4772985A (en) * | 1986-09-24 | 1988-09-20 | Kabushiki Kaisha Toshiba | Thick film capacitor |
| US4820670A (en) * | 1986-11-26 | 1989-04-11 | Murata Manufacturing Co., Ltd. | Dielectric ceramic composition |
| EP0413321B1 (en) * | 1989-08-17 | 1995-06-21 | Matsushita Electric Industrial Co., Ltd. | Dielectric ceramic composition and multi-layer capacitor |
| JPH03102705A (en) * | 1989-09-18 | 1991-04-30 | Murata Mfg Co Ltd | Dielectrics porcelain compound |
| US20050287085A1 (en) * | 2002-09-06 | 2005-12-29 | Dentsply International Inc. | Composition for improving the physico-chemical properties of apatite-based materials, uses thereof and method using same |
Family Cites Families (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS557713A (en) * | 1978-06-30 | 1980-01-19 | Furukawa Electric Co Ltd:The | Production of optical fiber aggregate |
| US4347167A (en) * | 1980-10-01 | 1982-08-31 | University Of Illinois Foundation | Fine-grain semiconducting ceramic compositions |
| US4379319A (en) * | 1982-02-18 | 1983-04-05 | Ferro Corporation | Monolithic ceramic capacitors and improved ternary ceramic compositions for producing same |
| JPS6020914B2 (en) * | 1983-04-21 | 1985-05-24 | 日本電気株式会社 | electrostrictive porcelain composition |
| US4542107A (en) * | 1983-05-30 | 1985-09-17 | Matsushita Electric Industrial Co., Ltd. | Dielectric ceramic compositions |
-
1984
- 1984-11-27 JP JP59250798A patent/JPS61128409A/en not_active Expired - Lifetime
-
1985
- 1985-11-23 DE DE19853541517 patent/DE3541517A1/en active Granted
- 1985-11-25 US US06/801,483 patent/US4601989A/en not_active Expired - Lifetime
- 1985-11-25 CA CA000496126A patent/CA1251037A/en not_active Expired
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5439857A (en) * | 1993-06-30 | 1995-08-08 | Murata Manufacturing Co., Ltd. | Dielectric ceramic composition |
Also Published As
| Publication number | Publication date |
|---|---|
| US4601989A (en) | 1986-07-22 |
| DE3541517A1 (en) | 1986-05-28 |
| DE3541517C2 (en) | 1993-04-01 |
| CA1251037A (en) | 1989-03-14 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| EXPY | Cancellation because of completion of term |